WO2022129533A1 - Ensemble de cellules électrochimiques, véhicule comprenant ledit ensemble et procédé de fabrication de l'ensemble - Google Patents

Ensemble de cellules électrochimiques, véhicule comprenant ledit ensemble et procédé de fabrication de l'ensemble Download PDF

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Publication number
WO2022129533A1
WO2022129533A1 PCT/EP2021/086505 EP2021086505W WO2022129533A1 WO 2022129533 A1 WO2022129533 A1 WO 2022129533A1 EP 2021086505 W EP2021086505 W EP 2021086505W WO 2022129533 A1 WO2022129533 A1 WO 2022129533A1
Authority
WO
WIPO (PCT)
Prior art keywords
gas diffusion
diffusion layer
catalyst
adhesive
bipolar plate
Prior art date
Application number
PCT/EP2021/086505
Other languages
German (de)
English (en)
Inventor
Andreas RINGK
Original Assignee
Robert Bosch Gmbh
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Robert Bosch Gmbh filed Critical Robert Bosch Gmbh
Publication of WO2022129533A1 publication Critical patent/WO2022129533A1/fr

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0286—Processes for forming seals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0297—Arrangements for joining electrodes, reservoir layers, heat exchange units or bipolar separators to each other
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • Electrochemical cell assembly vehicle comprising the assembly and method of making the assembly
  • the invention relates to an arrangement of electrochemical cells, comprising at least one gas diffusion layer, preferably with a microporous layer, a catalyst-coated membrane with a frame, and a bipolar plate. Furthermore, the invention relates to a vehicle comprising the arrangement and a method for producing the arrangement.
  • Electrochemical cells are electrochemical energy converters and are known in the form of fuel cells or electrolyzers.
  • a fuel cell converts chemical reaction energy into electrical energy.
  • known fuel cells in particular hydrogen (H2) and oxygen (O2) are converted into water (H2O), electrical energy and heat.
  • PEM proton exchange membranes
  • Fuel cells have an anode and a cathode.
  • the fuel is continuously fed to the anode of the fuel cell and is catalytically oxidized to protons with the release of electrons, which then reach the cathode.
  • the emitted electrons are drained from the fuel cell and flow via an external circuit to the cathode.
  • the oxidizing agent is supplied to the cathode of the fuel cell and reacts by absorbing the electrons from the external circuit and protons to form water. The resulting water is drained from the fuel cell.
  • the gross cathode reaction is:
  • a voltage between the anode and the cathode of the fuel cell There is a voltage between the anode and the cathode of the fuel cell.
  • several fuel cells can be arranged mechanically one behind the other to form a fuel cell stack, which is also referred to as a stack or fuel cell structure, and connected electrically in series.
  • a stack of electrochemical cells which may be referred to as an electrochemical cell array, typically has end plates that compress the individual cells together and provide stability to the stack.
  • the electrodes ie the anode and the cathode, and the membrane can be structurally combined.
  • Stacks of electrochemical cells also include bipolar plates, also referred to as gas distribution plates or distribution plates.
  • Bipolar plates are used to evenly distribute fuel to the anode and evenly distribute oxidant to the cathode.
  • the bipolar plates ensure a planar electrical contact with the membrane.
  • a fuel cell stack typically includes up to a few hundred individual fuel cells that are stacked on top of one another in layers.
  • the individual fuel cells have an MEA and a bipolar plate half on the anode side and on the cathode side.
  • a fuel cell includes in particular an anode monopolar plate and a cathode monopolar plate, usually each in the form of embossed metal sheets, which together form the bipolar plate and thus channels for conducting gas and liquids and between which the coolant can flow.
  • electrochemical cells typically include gas diffusion layers sandwiched between a bipolar plate and a membrane.
  • an electrolyser In contrast to a fuel cell, an electrolyser is an energy converter which splits water into hydrogen and oxygen when an electrical voltage is applied. Electrolyzers also have a membrane, bipolar plates and gas diffusion layers, among other things.
  • the membrane may have a thin layer of catalyst, so it is referred to as a catalyst coated membrane or Catalyst Coated Membrane (CCM).
  • CCM Catalyst Coated Membrane
  • the gas diffusion layers can each be bonded to a catalyst-coated membrane, forming a membrane-electrode assembly, which is also referred to as a membrane electrode assembly (MEA).
  • MEA membrane electrode assembly
  • the MEA is then typically placed on a bipolar plate to form the array of electrochemical cells, followed by stacking, also referred to as stacking.
  • DE 11 2005 002 974 B4 relates to a method for increasing the adhesive strength between elements of a fuel cell to be bonded, the elements to be bonded being subjected to a surface treatment.
  • DE 102 24452 CI is directed to a proton-conducting polymer membrane, with a catalyst layer being applied homogeneously to the polymer membrane.
  • the coated, proton-conducting polymer membrane is part of a membrane-electrode unit that has a gas distribution structure and a diffusion layer on the cathode and anode side.
  • a catalyst layer applied homogeneously to the polymer membrane is removed in regions in order to create catalyst segments which are separate from one another.
  • the gas diffusion layers often consist of carbon fiber materials which are bonded together using Teflon, with pure Teflon being very difficult to bond.
  • Carbon fibers, also known as carbon fibers, are also relatively difficult to bond, which is understood in particular that only a few adhesive forces can be formed.
  • DD 106 052 relates to a process for producing reinforced polymer moldings.
  • An arrangement of electrochemical cells comprising at least one gas diffusion layer, preferably with a microporous layer, a catalyst-coated membrane with a frame and a bipolar plate, the gas diffusion layer being connected to the catalyst-coated membrane and/or to the bipolar plate by means of an adhesive which Adhesive is arranged on a surface of the frame of the catalyst-coated membrane, the bipolar plate and/or optionally the microporous layer of the gas diffusion layer and the surface is plasma-functionalized.
  • a vehicle comprising the arrangement of electrochemical cells
  • a method for producing the arrangement of electrochemical cells comprising the following steps: a. providing at least one gas diffusion layer, preferably with a microporous layer, a catalyst-coated membrane with a frame and a bipolar plate, b. Pretreating a surface of the frame of the catalyst-coated membrane, the bipolar plate and/or optionally the microporous layer of the gas diffusion layer by means of plasma, in particular using shadow masks, so that a pretreated surface is produced, c. applying an adhesive to the pretreated surface of the frame of the catalyst-coated membrane, the bipolar plate and/or optionally the microporous layer of the gas diffusion layer, d. Stacking the gas diffusion layer, the catalyst coated membrane and the bipolar plate to form the electrochemical cell assembly.
  • the array of electrochemical cells is preferably a fuel cell stack.
  • the array of electrochemical cells includes at least one electrolyzer.
  • the arrangement of electrochemical cells preferably comprises at least two gas diffusion layers and at least two bipolar plates, with the catalyst-coated membrane preferably being arranged between the two bipolar plates and more preferably one gas diffusion layer being arranged between the catalyst-coated membrane and one of the bipolar plates.
  • the bipolar plate preferably comprises at least one port for the passage of at least one medium such as hydrogen, oxygen or a coolant and an active surface on which the electrochemical reaction takes place.
  • the arrangement of electrochemical cells can have at least one seal, with the bipolar plate preferably having the at least one seal. More preferably, the at least one seal surrounds the at least one port and the active area.
  • the port can be an inlet or an outlet for the at least one medium and the bipolar plate can comprise more than one port.
  • the bipolar plate preferably includes carbon such as graphite, a metal such as stainless steel or titanium and/or an alloy containing the metal. More preferably, the bipolar plate is made of carbon, the metal and/or the alloy.
  • the gas diffusion layer preferably includes the microporous layer, which is also referred to as the microporous layer (MPL). More preferably, the gas diffusion layer comprises a carbon fiber fleece, which is also referred to as "gas diffusion backing" (GDB), and in particular the gas diffusion layer consists of the carbon fiber fleece and the microporous layer.
  • GDB gas diffusion backing
  • the microporous layer is preferably located on a first side of the gas diffusion layer that faces the membrane.
  • the carbon fiber fleece is preferably arranged on a second side of the gas diffusion layer that faces the bipolar plate.
  • the microporous layer of the gas diffusion layer is preferably located adjacent to the catalyst coated membrane.
  • the microporous layer has a micropore structure, with the average pore size preferably being less than 1 ⁇ m. Further the microporous layer preferably has a layer thickness in a range from 1 ⁇ m to 100 ⁇ m.
  • the frame of the catalyst-coated membrane can also be referred to as a stiffener or gasket and preferably comprises a plastic material, in particular polyethylene naphthalate (PEN), more preferably the frame of the catalyst-coated membrane consists of the plastic material, in particular polyethylene naphthalate (PEN).
  • PEN polyethylene naphthalate
  • the gas diffusion layer in particular the microporous layer, preferably contains carbon fibers and optionally polytetrafluoroethylene, which is also referred to as Teflon.
  • the adhesive which can also be referred to as an adhesive, is preferably present as a coating on the surface.
  • the surface is in particular a part of the frame of the catalyst-coated membrane, the bipolar plate and/or optionally the microporous layer of the gas diffusion layer.
  • the adhesive is electrically conductive.
  • the adhesive preferably has a low contact resistance between the bipolar plate and the gas diffusion layer. More preferably, the transition resistance is in the order of 50 mm Ohm ⁇ cm 2 .
  • the adhesive may include an electrically conductive filler.
  • the adhesive consists of an adhesive material containing the electrically conductive filler.
  • a filler content is preferably between 5% and 95%, more preferably between 50% and 95%.
  • the adhesive, in particular the adhesive material preferably contains epoxy resin, acrylate, polyurethane, silicone, polyester or mixtures thereof.
  • the electrically conductive filler preferably comprises graphite and/or a metal such as silver. More preferably, the electrically conductive filler consists of graphite and/or the metal such as silver, in particular silver.
  • the adhesive can be a one-component adhesive or a two-component adhesive, and the adhesive can preferably be cured.
  • the curing of the adhesive is preferably carried out at a temperature in a range from 10°C to 90°C, more preferably from 15°C to 80°C.
  • a covalent connection of carbon fibers can take place, for example, via amine groups with an epoxide.
  • the pretreatment by means of plasma is carried out in particular in an atmosphere containing air, in particular oxygen.
  • the atmosphere may contain H2, N2, SO2, H2O and/or air, among others.
  • the plasma is preferably an NH3 plasma, oxygen plasma, nitrogen plasma or sulfur dioxide plasma. Nozzles of various designs can be used for pretreatment with plasma.
  • the pretreatment by means of plasma is preferably carried out immediately before the adhesive is applied. Shadow masks can be used here, so that the pre-treatment by means of plasma is only carried out in selected areas of the surface.
  • the adhesive is preferably first applied to the gas diffusion layer and/or the bipolar plate, then the gas diffusion layer and the bipolar plate are stacked one on top of the other and then the catalyst-coated membrane is placed on the gas diffusion layer. More preferably, the adhesive is first applied to two gas diffusion layers and the bipolar plate is arranged between the two gas diffusion layers with the adhesive, so that a bipolar plate with two bonded gas diffusion layers is present, on which the catalyst-coated membrane with the frame is then preferably placed and optionally on a stack is added.
  • the adhesive can first be applied to the bipolar plate, on which two gas diffusion layers are then arranged, so that a bipolar plate with two gas diffusion layers glued on is formed.
  • step c This is preferably followed by the application of the adhesive in step c. forming covalent bonds between the adhesive and the pretreated surface.
  • O2, F2, N2, Ar can be used as the process gas for dismantling and etching the surface, which is in particular a polymeric surface, with the surface being cleaned.
  • NH3, N2, SO2, H2O and/or air can be used as the process gas for functionalizing the surface, in particular for breaking down and crosslinking.
  • the surface is activated for gluing, painting, printing and chemical reactions.
  • the plasma functionality of the surface or the pretreatment of the surface by means of plasma achieves a covalent fixation of the adhesive to the frame of the membrane, the bipolar plate or the microporous layer of the gas diffusion layer, which represents a stronger material connection and thus a stronger fixation of the gas diffusion layer on the Bipolar plate or the catalyst-coated membrane is used. Furthermore, better wetting of the surface with the adhesive is possible.
  • the adhesive By using the adhesive, a pressing force which is usually required in the arrangement of electrochemical cells and which can impair the gas diffusion layer in particular, can be significantly reduced and thus gas distribution in the electrochemical cell can be improved.
  • the electrical contact between the bipolar plate and the gas diffusion layer is further improved by the electrically conductive adhesive. A transition resistance is reduced.
  • the adhesive prevents the gas diffusion layer or the catalyst-coated membrane from slipping on the bipolar plate when the arrangement is stacked.
  • FIG. 1 shows a fuel cell stack according to the prior art
  • FIG. 2 shows a schematic representation of a method for producing an arrangement of electrochemical cells according to the prior art
  • FIG. 3 shows a schematic representation of the method according to the invention for producing an arrangement of electrochemical cells.
  • FIG. 1 shows an arrangement of electrochemical cells 1 according to the prior art.
  • the arrangement of electrochemical cells 1 comprises a layering of bipolar plates 3 and gas diffusion layers 5.
  • a membrane 7 is also shown.
  • An electrical contact 17 is produced between a gas diffusion layer 5 and a bipolar plate 3 in each case by means of a contact pressure 15 .
  • Hydrogen 19 flows through the bipolar plates 3 on the one hand and air 21 and water 23 on the other hand, which each reach the membrane 7 through a gas diffusion layer 5 and are removed from it.
  • electrodes 25 are routed through the bipolar plates 3 .
  • FIG. 2 shows a schematic representation of a method for producing an arrangement of electrochemical cells 1 according to the prior art.
  • a catalyst-coated membrane 7 with a frame 43 is placed between two gas diffusion layers 5 so that a membrane-electrode assembly 2 is formed, which is placed on a bipolar plate 3 with a gasket 41 and ports 45 .
  • the bipolar plates 3 with membrane electrode assemblies 2 are then stacked to form an assembly of electrochemical cells 1 .
  • FIG. 3 shows a schematic representation of a method according to the invention for producing an arrangement of electrochemical cells 1.
  • Two Gas diffusion layers 5 are partially provided with an adhesive 9 after a mesoporous layer of the gas diffusion layers 5 has been pretreated by means of plasma.
  • a bipolar plate 3 with a seal 41 is arranged between the gas diffusion layers 5, which have the adhesive 9, and is bonded to the gas diffusion layers 5 by the adhesive 9.
  • a bipolar plate 3 that already has a seal 41 can be partially provided with the adhesive 9 after a surface 8 of a microporous layer of the gas diffusion layers 5 has been pretreated with plasma. Then two gas diffusion layers 5 can be arranged on either side of the bipolar plate 3 .
  • a catalyst-coated membrane 7 with a frame 43 is placed on the gas diffusion layer 5 and a plurality of bipolar plates 3 with gas diffusion layers 5 and catalyst-coated membranes 7 are stacked to form the electrochemical cell arrangement 1 .

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  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Fuel Cell (AREA)

Abstract

L'invention concerne un ensemble de cellules électrochimiques (1), comprenant au moins une couche de diffusion de gaz (5), de préférence avec une couche microporeuse, une membrane revêtue de catalyseur (7) avec un cadre (43), et une plaque de champ d'écoulement (3), la couche de diffusion de gaz (5) étant jointe à la membrane revêtue de catalyseur (8) et/ou à la plaque de champ d'écoulement (3) au moyen d'un adhésif (9) qui est disposé sur une surface (8) du cadre (43) de la membrane revêtue de catalyseur (7), la plaque de champ d'écoulement (3) et/ou, le cas échéant, la couche microporeuse de la couche de diffusion de gaz (5), la surface (8) étant fonctionnalisée par plasma. L'invention concerne en outre un véhicule comprenant ledit ensemble de cellules électrochimiques (1) et un procédé de fabrication d'un ensemble de cellules électrochimiques (1).
PCT/EP2021/086505 2020-12-17 2021-12-17 Ensemble de cellules électrochimiques, véhicule comprenant ledit ensemble et procédé de fabrication de l'ensemble WO2022129533A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102020216101.1 2020-12-17
DE102020216101.1A DE102020216101A1 (de) 2020-12-17 2020-12-17 Anordnung elektrochemischer Zellen, Fahrzeug umfassend die Anordnung und Verfahren zur Herstellung der Anordnung

Publications (1)

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WO2022129533A1 true WO2022129533A1 (fr) 2022-06-23

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DE (1) DE102020216101A1 (fr)
WO (1) WO2022129533A1 (fr)

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DD106052A1 (fr) 1972-11-08 1974-05-20
DE10224452C1 (de) 2002-05-29 2003-11-20 Fraunhofer Ges Forschung Protonenleitende Polymermembran sowie Verfahren zu deren Herstellung
DE112005002974T5 (de) * 2004-12-13 2007-10-25 General Motors Corp., Detroit Konstruktion, Verfahren und Prozess für eine vereinheitlichte MEA
DE102010028957A1 (de) * 2010-05-12 2011-11-17 Trumpf Werkzeugmaschinen Gmbh + Co. Kg Brennstoffzellenstapel und Verfahren zum Herstellen eines Brennstoffzellenstapels
US20160285119A1 (en) * 2013-12-10 2016-09-29 Toyota Jidosha Kabushiki Kaisha Power generation body (as amended)
CN111509259A (zh) * 2020-04-14 2020-08-07 上海神力科技有限公司 一种提高燃料电池极板表面粘合剂稳定性的方法

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DD106052A1 (fr) 1972-11-08 1974-05-20
DE10224452C1 (de) 2002-05-29 2003-11-20 Fraunhofer Ges Forschung Protonenleitende Polymermembran sowie Verfahren zu deren Herstellung
DE112005002974T5 (de) * 2004-12-13 2007-10-25 General Motors Corp., Detroit Konstruktion, Verfahren und Prozess für eine vereinheitlichte MEA
DE112005002974B4 (de) 2004-12-13 2010-03-04 General Motors Corp., Detroit Verfahren zum Erhöhen der Klebkraft zwischen mittels eines Klebstoffs zu verbindenden Elementen einer Brennstoffzellen-Membranelektrodenanordnung
DE102010028957A1 (de) * 2010-05-12 2011-11-17 Trumpf Werkzeugmaschinen Gmbh + Co. Kg Brennstoffzellenstapel und Verfahren zum Herstellen eines Brennstoffzellenstapels
US20160285119A1 (en) * 2013-12-10 2016-09-29 Toyota Jidosha Kabushiki Kaisha Power generation body (as amended)
CN111509259A (zh) * 2020-04-14 2020-08-07 上海神力科技有限公司 一种提高燃料电池极板表面粘合剂稳定性的方法

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